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Sökning: AMNE:(NATURAL SCIENCES Chemistry Environmental chemistry)

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51.
  • Donahue, N. M., et al. (författare)
  • Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions
  • 2012
  • Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 109:34, s. 13503-13508
  • Tidskriftsartikel (refereegranskat)abstract
    • The Multiple Chamber Aerosol Chemical Aging Study (MUCHACHAS) tested the hypothesis that hydroxyl radical (OH) aging significantly increases the concentration of first-generation biogenic secondary organic aerosol (SOA). OH is the dominant atmospheric oxidant, and MUCHACHAS employed environmental chambers of very different designs, using multiple OH sources to explore a range of chemical conditions and potential sources of systematic error. We isolated the effect of OH aging, confirming our hypothesis while observing corresponding changes in SOA properties. The mass increases are consistent with an existing gap between global SOA sources and those predicted in models, and can be described by a mechanism suitable for implementation in those models.
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52.
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53.
  • Rämö, Robert, et al. (författare)
  • Sediment Remediation Using Activated Carbon: Effects of Sorbent Particle Size and Resuspension on Sequestration of Metals and Organic Contaminants.
  • 2022
  • Ingår i: Environmental toxicology and chemistry. - : Wiley. - 1552-8618 .- 0730-7268. ; 41:4, s. 1096-1110
  • Tidskriftsartikel (refereegranskat)abstract
    • Thin-layer capping using activated carbon (AC) has been described as a cost-effective in situ sediment remediation method for organic contaminants. In this study, we compare the capping efficiency of powdered AC (PAC) against granular AC (GAC) using contaminated sediment from Oskarshamn harbor, Sweden. The effects of resuspension on contaminant retention and cap integrity were also studied. Intact sediment cores were collected from the outer harbor and brought to the laboratory. Three thin-layer caps, consisting of PAC or GAC mixed with clay, or clay only, were added to the sediment surface. Resuspension was created using a motor-driven paddle to simulate propeller wash from ship traffic. Passive samplers were placed in the sediment and in the water column to measure the sediment-to-water release of PAHs, PCBs, and metals. Our results show that a thin-layer cap with PAC reduced sediment-to-water fluxes of PCBs by 57 % under static conditions and 91 % under resuspension. Thin-layer capping with GAC was less effective than PAC, but reduced fluxes of high-molecular weight PAHs. Thin-layer capping with AC was less effective in retaining metals, except for Cd, which release was significantly reduced by PAC. Resuspension generally decreased water concentrations of dissolved cationic metals, perhaps due to sorption to suspended sediment particles. Sediment resuspension in treatments without capping increased fluxes of PCBs with log Kow > 7 and PAHs with log Kow 5 6, but resuspension reduced PCB and PAH fluxes through the PAC thin-layer cap. Overall, PAC performed better than GAC, but adverse effects on the benthic community and transport of PAC to non-target areas are drawbacks that favor the use of GAC. This article is protected by copyright. All rights reserved.© 2022 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.
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54.
  • Hammes, Julia, et al. (författare)
  • Carboxylic acids from limonene oxidation by ozone and hydroxyl radicals: insights into mechanisms derived using a FIGAERO-CIMS
  • 2019
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:20, s. 13037-13052
  • Tidskriftsartikel (refereegranskat)abstract
    • This work presents the results from a flow reactor study on the formation of carboxylic acids from limonene oxidation in the presence of ozone under NOx-free conditions in the dark. A High-Resolution Time-of-Flight acetate Chemical Ionisation Mass Spectrometer (HR-ToF-CIMS) was used in combination with a Filter Inlet for Gases and AEROsols (FIGAERO) to measure the carboxylic acids in the gas and particle phases. The results revealed that limonene oxidation produced large amounts of carboxylic acids which are important contributors to secondary organic aerosol (SOA) formation. The highest 10 acids contributed 56 %-91 % to the total gas-phase signal, and the dominant gas-phase species in most experiments were C8H12O4, C9H14O4, C7H10O4 and C10H16O3. The particle-phase composition was generally more complex than the gas-phase composition, and the highest 10 acids contributed 47 %-92 % to the total signal. The dominant species in the particle phase were C8H12O5, C9H14O5, C9H12O5 and C10H16O4. The measured concentration of dimers bearing at least one carboxylic acid function in the particle phase was very low, indicating that acidic dimers play a minor role in SOA formation via ozone (O-3)/hydroxyl (OH) oxidation of limonene. Based on the various experimental conditions, the acidic compositions for all experiments were modelled using descriptions from the Master Chemical Mechanism (MCM). The experiment and model provided a yield of large (C-7-C-10) carboxylic acid of the order of 10 % (2 %-23 % and 10 %-15 %, respectively). Significant concentrations of 11 acids, from a total of 16 acids, included in the MCM were measured with the CIMS. However, the model predictions were, in some cases, inconsistent with the measurement results, especially regarding the OH dependence. Reaction mechanisms are suggested to fill-in the knowledge gaps. Using the additional mechanisms proposed in this work, nearly 75 % of the observed gas-phase signal in our lowest concentration experiment (8.4 ppb converted, ca. 23 % acid yield) carried out under humid conditions can be understood.
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55.
  • Wang, Y. J., et al. (författare)
  • Comparative Study of Particulate Organosulfates in Contrasting Atmospheric Environments: Field Evidence for the Significant Influence of Anthropogenic Sulfate and NOx
  • 2020
  • Ingår i: Environmental Science & Technology Letters. - : American Chemical Society (ACS). - 2328-8930. ; 7:11, s. 787-794
  • Tidskriftsartikel (refereegranskat)abstract
    • Organosulfates (OSs) are an important group of secondary organic aerosols, but the key influential factors of their formation in polluted atmospheres are not well understood. In this study, we monitored particulate OSs (carboxy OSs, hydroxyacetone sulfate, and isoprene- and monoterpene-derived OSs) at an urban site and a regional site in Beijing and examined their compositions and formation pathways under contrasting atmospheric conditions. The quantified OSs were most abundant in the summer at the regional site due to higher biogenic emissions and favorable formation conditions (higher aerosol acidity and humidity), followed by urban summer and winter conditions. Larger fractions of inorganic sulfate were converted to organosulfur when sulfate was less abundant. This implies that OSs would play more important roles in aerosol properties as the decline of sulfate. Monoterpene-derived nitrooxy-OSs were enhanced via NO3 oxidation in the summer under high-NOx conditions at night, while the day-night variations in the winter were not as obvious. Among isoprene-OSs, IEPOX (isoprene epoxydiols)-OS formation was clearly suppressed under high-NOx conditions, while other isoprene-OSs that are favored under high-NOx conditions showed increasing formation with NOx. The results highlight that isoprene-OS formation pathways in polluted atmospheres could be different from the IEPOX-dominated regions reported for the low-NOx environments in the literature.
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56.
  • Zhao, D. F., et al. (författare)
  • Size-dependent hygroscopicity parameter (κ) and chemical composition of secondary organic cloud condensation nuclei
  • 2015
  • Ingår i: Geophysical Research Letters. - 1944-8007. ; 42:24
  • Tidskriftsartikel (refereegranskat)abstract
    • Secondary organic aerosol components (SOA) contribute significantly to the activation of cloud condensation nuclei (CCN) in the atmosphere. The CCN activity of internally mixed submicron SOA particles is often parameterized assuming a size-independent single-hygroscopicity parameter κ. In the experiments done in a large atmospheric reactor (SAPHIR, Simulation of Atmospheric PHotochemistry In a large Reaction chamber, Jülich), we consistently observed size-dependent κ and particle composition for SOA from different precursors in the size range of 50 nm–200 nm. Smaller particles had higher κ and a higher degree of oxidation, although all particles were formed from the same reaction mixture. Since decreasing volatility and increasing hygroscopicity often covary with the degree of oxidation, the size dependence of composition and hence of CCN activity can be understood by enrichment of higher oxygenated, low-volatility hygroscopic compounds in smaller particles. Neglecting the size dependence of κ can lead to significant bias in the prediction of the activated fraction of particles during cloud formation.
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57.
  • Finlay, Roger, et al. (författare)
  • The role of fungi in biogenic weathering in boreal forest soils
  • 2009
  • Ingår i: Fungal Biology Reviews. - : Elsevier. - 1749-4613 .- 1878-0253. ; 23:4, s. 101-106
  • Tidskriftsartikel (refereegranskat)abstract
    • In this article we discuss the possible significance of biological processes, and of fungi in particular, in weathering of minerals. We consider biological activity to be a significant driver of mineral weathering in forest ecosystems. In these environments fungi play key roles in organic matter decomposition, uptake, transfer and cycling of organic and inorganic nutrients, biogenic mineral formation, as well as transformation and accumulation of metals. The ability of lichens, mutualistic symbioses between fungi and photobionts such as algae or cyanobacteria, to weather minerals is well documented. The role of mycorrhizal fungi forming symbioses with forest trees is less well understood, but the mineral horizons of boreal forests are intensively colonised by mycorrhizal mycelia which transfer protons and organic metabolites derived from plant photosynthates to mineral surfaces, resulting in mineral dissolution and mobilisation and redistribution of anionic nutrients and metal cations. The mycorrhizal mycelia, in turn provide efficient systems for the uptake and direct transport of mobilised essential nutrients to their host plants which are large sinks. Since almost all (99.99. %) non-suberised lateral plant roots involved in nutrient uptake are covered by ectomycorrhizal fungi, most of this exchange of metabolites must take place through the plant-fungus interface. This idea is still consistent with a linear relationship between soil mineral surface area and weathering rate since the mycelia that emanate from the tree roots will have a larger area of contact with minerals if the mineral surface area is higher. Although empirical models based on bulk soil solution chemistry may fit field data, we argue that biological processes make an important contribution to mineral weathering and that a more detailed mechanistic understanding of these must be developed in order to predict responses to environmental changes and anthropogenic impact. © 2010 The British Mycological Society.
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58.
  • Gunnarsson, Lina-Maria, 1977, et al. (författare)
  • Comparison of six different sewage treatment processes-Reduction of estrogenic substances and effects on gene expression in exposed male fish
  • 2009
  • Ingår i: Science of the Total Environment. - : Elsevier. - 0048-9697 .- 1879-1026. ; 407:19, s. 5235-5242
  • Tidskriftsartikel (refereegranskat)abstract
    • Treated sewage effluents often contain a mixture of estrogenic compounds in low concentrations. The total combined activity of these, however, may be sufficiently high to affect the reproduction of aquatic vertebrates. The introduction of advanced treatment technologies has been suggested as a way to remove micro-contaminants, including estrogenic substances. In this study, one municipal influent was treated with six different processes in parallel on a semi-large scale in order to assess their potential to reduce substances that could contribute to estrogenic effects in male fish. The effluent from a conventional, activated sludge treatment line was compared to a similarly treated effluent with a final sand-filtering step. The addition of ozonation (15 g O-3/m(3)). a moving bed biofilm reactor (MBBR) or both in combination was also evaluated. There was also a separate treatment line that was based on a membrane bioreactor. A small battery of hepatic estrogen-responsive genes was measured in the exposed fish using quantitative PCR. Concentrations of steroid estrogens and estrogenic phenols in the effluents were measured by GC-ECNI-MS. The ozonated effluents were the only tested effluents for which all measured biological effects in exposed fish were removed. Chemical data suggested that the MBBR technology was equally effective in removing the analyzed estrogens; however, elevated expression of estrogen-responsive genes suggested that some estrogenic substances were still present in the effluent. The membrane bioreactor removed most of the measured estrogens and it reduced the induction of the estrogen-responsive genes. However, fish exposed to this effluent had significantly enlarged livers. Given that the same influent was treated in parallel with a broad set of technologies and that the chemical analyses were combined with an in vivo assessment of estrogenic responses, this study provides valuable input into the assessment of advanced treatment processes for removing estrogenic substances.
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59.
  • Elgh-Dalgren, Kristin, et al. (författare)
  • Anaerobic bioremediation of a soil with mixed contaminants : Explosives degradation and influence on heavy metal distribution, monitored as changes in concentration and toxicity
  • 2009
  • Ingår i: Water, Air and Soil Pollution. - Dordrecht : Springer Netherlands. - 0049-6979 .- 1573-2932. ; 202:1-4, s. 301-313
  • Tidskriftsartikel (refereegranskat)abstract
    • Two soils with explosives and metals were evaluated for the degradation efficiency of explosives by native microorganisms under anaerobic conditions. The commercially available method Daramend®, amended with zero-valent iron (ZVI), was compared with a horse-manure amended compost and a treatment with ZVI alone. In a moderately contaminated soil, Daramend® and ZVI treatment gave significantly higher removal rates compared  to compost and control treatments (Tukey’s test, P<0.05). The largest overall decrease in ecotoxicity, measured with bioluminescent bacteria (Vibrio fischeri), was achieved with ZVI-treatment. In a more contaminated soil no degradation of contaminants and no decline in soil toxicity could be distinguished after the same time period. Problems with establishment of anaerobic conditions during parts of the remediation process and low microbial activity due to acute toxicity of contaminants are plausible explanations. Redistribution that could potentially lead to mobilization of the co-contaminant Pb was not observed in either of the soils during the biological treatments.
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60.
  • Wang, H. C., et al. (författare)
  • Efficient N2O5 uptake and NO3 oxidation in the outflow of urban Beijing
  • 2018
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:13, s. 9705-9721
  • Tidskriftsartikel (refereegranskat)abstract
    • Nocturnal reactive nitrogen compounds play an important role in regional air pollution. Here we present the measurements of dinitrogen pentoxide (N2O5) associated with nitryl chloride (ClNO2) and particulate nitrate (pNO(3)(-)) at a suburban site of Beijing in the summer of 2016. High levels of N2O5 and ClNO2 were observed in the outflow of the urban Beijing air masses, with 1 min average maxima of 937 and 2900 pptv, respectively. The N2O5 uptake coefficients, gamma, and ClNO2 yield, f, were experimentally determined from the observed parameters. The N2O5 uptake coefficient ranged from 0.012 to 0.055, with an average of 0.034 +/- 0.018, which is in the upper range of previous field studies reported in North America and Europe but is a moderate value in the North China Plain (NCP), which reflects efficient N2O5 heterogeneous processes in Beijing. The ClNO2 yield exhibited high variability, with a range of 0.50 to unity and an average of 0.73 +/- 0.25. The concentration of the nitrate radical (NO3) was calculated assuming that the thermal equilibrium between NO3 and N2O5 was maintained. In NOx-rich air masses, the oxidation of nocturnal biogenic volatile organic compounds (BVOCs) was dominated by NO3 rather than O-3. The production rate of organic nitrate (ON) via NO3 + BVOCs was significant, with an average of 0.10 +/- 0.07 ppbvh(-1). We highlight the importance of NO3 oxidation of VOCs in the formation of ON and subsequent secondary organic aerosols in summer in Beijing.
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